We explore the dynamics of entangled polymer chains embedded into nanocomposites. From primitive path analysis, highly entangled polymer chains are found to be significantly disentangled during increment of the volume fraction of spherical nonattractive nanoparticles (NPs) from 0 to 42%. A critical volume fraction, ϕ(c)=31%, is found to control the crossover from polymer chain entanglements to "NP entanglements." While below ϕ(c), the polymer chain relaxation accelerates upon filling, above ϕ(c), the situation reverses: polymer dynamics becomes geometrically constrained upon adding NPs. Our findings provide a microscopic understanding of the dynamics of entangled polymer chains inside their composites, and offer an explanation for the unusual rheological properties of polymer composites.

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Assembling Ti3C2T x MXene nanosheets into three-dimensional (3D) architecture with controllable alignment is of great importance for electromagnetic wave absorption (EMA) application. However, it is a great challenge to realize it due to the weak van der Waals interconnection between MXene nanosheets. Herein, we propose to introduce gelatin molecules as a “chemical glue” to fabricate the 3D Mxene@gelatin (M@G) nanocomposite aerogel using a unidirectional freeze casting method. The Ti3C2T x MXene nanosheets are well aligned in the M@G nanocomposite aerogel, yielding much enhanced yet anisotropic mechanical properties. Due to the unidirectional aligned microstructure, the M@G nanocomposite aerogel shows significantly anisotropic EMA properties. M@G-45 shows a −59.5 dB minimum reflection loss (RLmin) at 14.04 GHz together with a 6.24 GHz effective absorption bandwidth in the parallel direction (relative to the direction of unidirectional freeze casting). However, in the vertical direction of the same M@G aerogel, RLmin is shifted to a much lower frequency (4.08 GHz) and the effective absorption bandwidth decreases to 0.86 GHz. The anisotropic electromagnetic energy dissipation mechanism was deeply investigated, and the impendence match plays a critical role for electromagnetic wave penetration. Our lightweight M@G nanocomposite aerogel with controllable MXene alignment is very promising in EMA application.

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Optical ignition of solid energetic materials, which can rapidly release heat, gas, and thrust, is still challenging due to the limited light absorption and high ignition energy of typical energetic materials (e.g., aluminum, Al). Here, we demonstrated that the optical ignition and combustion properties of micron-sized Al particles were greatly enhanced by adding only 20 wt % of graphene oxide (GO). These enhancements are attributed to the optically activated disproportionation and oxidation reactions of GO, which release heat to initiate the oxidization of Al by air and generate gaseous products to reduce the agglomeration of the composites and promote the pressure rise during combustion. More importantly, compared to conventional additives such as metal oxides nanoparticles (e.g., WO 3 and Bi 2 O 3 ), GO has much lower density and therefore could improve energetic properties without sacrificing Al content. The results from Xe flash ignition and laser-based excitation experiments demonstrate that GO is an efficient additive to improve the energetic performance of micron-sized Al particles, enabling micron-sized Al to be ignited by optical activation and promoting the combustion of Al in air.

Hydrogenation of carbon−oxygen bonds is extensively used in organic synthesis. However, a high partial pressure of hydrogen or the presence of excess hydrogen is usually essential to achieve favorable conversions. In addition, because most hydrogenations are consecutive reactions, the selectivity is difficult to manipulate, leading to an unsatisfactory distribution of products. Herein, a copper silicate nanoreactor with a nanotube-assembled hollow sphere (NAHS) hierarchical structure is proposed as a solution to these problems. In the case of dimethyl oxalate (DMO) hydrogenation, the NAHS nanoreactor achieves remarkable catalytic activity (the yield of ethylene glycol is 95%) and stability (>300 h) when the H 2 / DMO molar ratio is as low as 20 (in comparison to typical values of 80−200). For further investigation, nanotubes and lamellarshaped Cu/SiO 2 catalysts with similar surface areas of active sites of NAHSs were investigated as contrasts. By a combination of high-pressure hydrogen adsorption and Monte Carlo simulation, it is demonstrated that hydrogen can be enriched on the concave surface of nanotubes and hollow spheres, leading to a favorable activity in such a low H 2 proportion. Furthermore, because of the spatial restriction effect of reactants, adjusting the diffusion path is an effective route for manipulating the selectivity and product distribution of the hydrogenation reactions. By variation in the length of nanotubes on NAHS, the yields of methyl glycolate and ethylene glycol are easily controlled. The NAHS nanoreactor, with insights into the effect of morphology on hydrogen enrichment and spatial restriction of reactant diffusion, offers inspiring possibilities in the rational design of catalysts for hydrogenation reactions.

Conductive hydrogel-based wearable strain sensors with tough, stretchable, self-recoverable, and highly sensitive properties are highly demanded for applications in electronic skin and human–machine interface. However, currently, hydrogel-based strain sensors put forward higher requirements on their biocompatibility, mechanical strength, and sensitivity. Herein, we report a poly­(vinyl alcohol)/phytic acid/amino-polyhedral oligomeric silsesquioxane (PVA/PA/NH2-POSS) conductive composite hydrogel prepared via a facile freeze–thaw cycle method. Within this hydrogel, PA acts as a cross-linking agent and ionizes hydrogen ions to endow the material with ionic conductivity, while NH2-POSS acts as a second cross-linking agent by increasing the cross-linking density of the three-dimensional network structure. The effect of the content of NH2-POSS is investigated, and the composite hydrogel with 2 wt % NH2-POSS displays a uniform and dense three-dimensional (3D) network microporous structure, high conductivity of 2.41 S/m, and tensile strength and elongation at break of 361 kPa and 363%, respectively. This hydrogel is biocompatible and has demonstrated the application as a strain sensor monitoring different human movements. The assembled sensor is stretchable, self-recoverable, and highly sensitive with fast response time (220 ms) and excellent sensitivity (GF = 3.44).

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